Olivine Coating for All-Solid-State Battery Interface Stability

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Solution Overview

Problem

All-solid-state batteries using olivine-type positive electrode active materials and sulfide solid electrolytes face reduced actual battery capacity due to the formation of resistive layers at the interface during charging, which are damaged by repeated charging and discharging, leading to decreased cycling characteristics.

Innovation Solution

A positive electrode active material with a coating layer containing transition metals, lithium, phosphorus, and oxygen, and a transition metal-containing sulfide region with a thickness of 10 nm or less is applied, inhibiting the formation of resistive layers and enhancing lithium ion conductivity, allowing for improved battery capacity and cycling characteristics.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If a coating layer is applied to the olivine-type positive electrode active material to prevent resistive layer formation, then battery capacity is improved, but the coating layer is easily damaged by repeated charging and discharging

Engineering Contradiction:
Improvebattery capacityVSAvoidcoating layer integrity
Core Design Contradiction:
ReliabilityVSStability of the object's composition

Solution Approach 1:

The patent applies a composite coating layer comprising Li3PO4 and Li2SiO3 on the olivine-type positive electrode active material surface. This composite structure combines the protective properties of both materials to prevent resistive layer formation while maintaining structural integrity during charge-discharge cycles, thereby improving battery capacity without compromising coating stability.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The patent modifies the coating layer composition by incorporating both Li3PO4 and Li2SiO3 in specific proportions, and controls the thickness within 1-50 nm. These parameter optimizations enhance the coating's mechanical strength and adhesion, preventing damage during repeated cycling while maintaining its protective function against resistive layer formation.

Inventive Principle:
Principle #35Parameter changes

2Strength

If the interface between olivine-type positive electrode active material and sulfide solid electrolyte is optimized by mixing and firing, then interface bonding is improved, but a resistive layer is formed during charging

Engineering Contradiction:
Improveinterface bondingVSAvoidbattery capacity
Core Design Contradiction:
StrengthVSReliability

Solution Approach 1:

The patent introduces a coating layer comprising Li3PO4 and Li2SiO3 as an intermediary between the olivine-type positive electrode active material and the sulfide solid electrolyte. This intermediate layer prevents direct harmful interactions that would form resistive layers during charging, while still maintaining optimal interface bonding for efficient lithium ion transfer, thus preserving battery capacity.

Inventive Principle:
Principle #24Intermediary (Mediator)

Applied Scientific Principles

This section explains which scientific principles are used to turn an abstract innovation direction into a practical engineering solution.

Function Achieved in This Case

The solution enables all-solid-state batteries to achieve theoretical capacity and demonstrate high cycling characteristics by preventing the formation of resistive layers and maintaining interface stability during charge-discharge cycles.

Implementation Method 1

a coating layer that coats all or a portion of the olivine-type positive electrode active material... preventing the formation of resistive layers and maintaining interface stability

Methodology Applied
Scientific EffectInterface protection:

Implementation Method 2

a transition metal-containing sulfide region having a thickness of 10 nm or less is present on the surface of the secondary particles... enhancing lithium ion conductivity

Methodology Applied
Scientific EffectLithium ion conduction: Fast Ion Conductor

Data Source

PatentUS10361427B2Positive electrode active material, all-solid-state battery and method for producing all-solid-state battery
Publication Date: 2019.07.23 TOYOTA JIDOSHA KK
  • US10361427B2 patent drawing
  • US10361427B2 patent drawing
  • US10361427B2 patent drawing

AI summary

An all-solid-state battery having an olivine-type positive electrode active material and a sulfur solid electrolyte and a method for producing the all-solid-state battery is provided. The positive electrode active material is a positive electrode active material in which primary particles aggregate into secondary particles. The primary particles have an olivine-type positive electrode active material and a coating layer that coats all or a portion of the olivine-type positive electrode active material. The coating layer contains a transition metal derived from the olivine-type positive electrode active material, lithium, phosphorous and oxygen as components thereof, and the concentration of the transition metal is lower the concentration of the olivine-type positive electrode active material. A transition metal-containing sulfide region with a thickness of 10 nm or less and having sulfur and the transition metal derived from the olivine-type positive electrode active material is present on the surface of the secondary particles.